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Surface tension predictions of hydrocarbon mixtures at vapour-liquid equilibrium are crucially important and used in the design of many unit operations in the production of liquefied natural gas (LNG). Predictive models for surface tension are not well tested for hydrocarbon mixtures at high pressures due to the limited data available at relevant conditions. A differential capillary rise apparatus consisting of a high-pressure sapphire equilibrium cell was constructed and used to measure the surface tension of methane + propane mixtures along three isotherms T = (272.23, 285.51 and 303.34) K at pressures up to 9 MPa. The capillary diameters were calibrated using pure saturated propane at 271 K, and the technique was validated by measurements of pure ethane. The measured surface tensions were compared with the available data and the predictions of various models, including the Parachor method and Linear Gradient Theory: both were able to describe the data within their uncertainty. However, the default surface tension model for hydrocarbon mixtures implemented in the widely-used software package REFPROP 9.1 gave poor predictions; this was rectified through the implementation of the Parachor method in a beta-version of REFPROP 9.2. Critical points were also measured from observations of critical opalescence and the disappearance of the bulk interface. The measured mixture critical points were consistent with, and extended, literature values for this binary system. The measured critical points differed by between 0.5 and +27 K from predictions made with the GERG-2008 equation of state (EOS) and between −5 and +10 K for the Peng-Robinson EOS.